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NASA NTRS2006

Quantum Entanglement Molecular Absorption Spectrum Simulator

Quantum Entanglement Molecular Absorption Spectrum Simulator (QE-MASS) is a computer program for simulating two photon molecular-absorption spectroscopy using quantum-entangled photons. More specifically, QE-MASS simulates the molecular absorption of two quantum-entangled photons generated by the spontaneous parametric down-conversion (SPDC) of a fixed-frequency photon from a laser. The two-photon absorption process is modeled via a combination of rovibrational and electronic single-photon transitions, using a wave-function formalism. A two-photon absorption cross section as a function of the entanglement delay time between the two photons is computed, then subjected to a fast Fourier transform to produce an energy spectrum. The program then detects peaks in the Fourier spectrum and displays the energy levels of very short-lived intermediate quantum states (or virtual states) of the molecule. Such virtual states were only previously accessible using ultra-fast (femtosecond) laser systems. However, with the use of a single-frequency continuous wave laser to produce SPDC photons, and QEMASS program, these short-lived molecular states can now be studied using much simpler laser systems. QE-MASS can also show the dependence of the Fourier spectrum on the tuning range of the entanglement time of any externally introduced optical-path delay time. QE-MASS can be extended to any molecule for which an appropriate spectroscopic database is available. It is a means of performing an a priori parametric analysis of entangled photon spectroscopy for development and implementation of emerging quantum-spectroscopic sensing techniques. QE-MASS is currently implemented using the Mathcad software package.

Nguyen, Quang-Viet↗

NASA NTRS2011

Analysis of Pulsed Airborne Lidar Measurements of Atmospheric CO2 Column Absorption from 3-13 km Altitudes

We have developed a pulsed lidar technique for measuring the tropospheric CO2 concentrations as a candidate for NASA's ASCENDS space mission [1]. It uses two pulsed laser transmitters allowing simultaneous measurement of a CO2 absorption line in the 1575 nm band, O2 extinction in the Oxygen A-band, surface height and backscatter profile. The lasers are precisely stepped in wavelength across the CO2 line and an O2 line region during the measurement. The direct detection receiver measures the energies of the laser echoes from the surface along with the range profile of scattering in the path. The column densities for the CO2 and O2 gases are estimated from the ratio of the on- and off-line signals via the integrated path differential absorption (IPDA) technique. The time of flight of the laser pulses is used to estimate the height of the scattering surface and to reject laser photons scattered in the atmosphere. We developed an airborne lidar to demonstrate an early version of the CO2 measurement from the NASA Glenn Lear-25 aircraft. The airborne lidar stepped the pulsed laser's wavelength across the selected CO2 line with 20 wavelength steps per scan. The line scan rate is 450 Hz, the laser pulse widths are 1 usec, and laser pulse energy is 24 uJ. The time resolved laser backscatter is collected by a 20 cm telescope, detected by a NIR photomultiplier and is recorded on every other reading by a photon counting system [2]. During August 2009 we made a series of 2.5 hour long flights and measured the atmospheric CO2 absorption and line shapes using the 1572.33 nm CO2 line. Measurements were made at stepped altitudes from 3-13 km over locations in the US, including the SGP ARM site in Oklahoma, central Illinois, north-eastern North Carolina, and over the Chesapeake Bay and the eastern shore of Virginia. Although the received signal energies were weaker than expected for ASCENDS, clear CO2 line shapes were observed at all altitudes, and some measurements were made through thin clouds. The Oklahoma and east coast flights were coordinated with a LaRC/ITT CO2 lidar on the LaRC UC-12 aircraft, and in-situ measurements were made using its CO2 sensor and radiosondes. We have conducted an analysis of the ranging and IPDA lidar measurements from these four flights. Most flights had 5-6 altitude steps with 200-300 seconds of recorded measurements per step. We used a cross-correlation approach to process the laser echo records. This was used to estimate the range to the scattering surface, to define the edges of the laser pulses and to determine echo pulse energy at each wavelength. We used a minimum mean square approach to fit an instrument response function and to solve for the best-fit CO2 absorption line shape. We then calculated the differential optical depth (DOD) of the fitted CO2 line. We computed its statistics at the various altitude steps, and compare them to the DODs calculated from spectroscopy based on HITRAN 2008 and the column conditions calculated from the airborne in-situ readings. The results show the lidar and in-situ measurements have very similar DOD change with altitude and greater than 10 segments per flight where the scatter in the lidar measurements are less than or equal to 1ppm. We also present the results from subsequent CO2 column absorption measurements, which were made with stronger detected signals during three flights on the NASA DC-8 over the southwestern US in during July 2010.

Abshire, James B.↗

NASA NTRS2012

An Analysis of AERONET Aerosol Absorption Properties and Classifications Representative of Aerosol Source Regions

Partitioning of mineral dust, pollution, smoke, and mixtures using remote sensing techniques can help improve accuracy of satellite retrievals and assessments of the aerosol radiative impact on climate. Spectral aerosol optical depth (tau) and single scattering albedo (omega (sub 0) ) from Aerosol Robotic Network (AERONET) measurements are used to form absorption [i.e., omega (sub 0) and absorption Angstrom exponent (alpha(sub abs))] and size [i.e., extinction Angstrom exponent (alpha(sub ext)) and fine mode fraction of tau] relationships to infer dominant aerosol types. Using the long-term AERONET data set (1999-2010), 19 sites are grouped by aerosol type based on known source regions to: (1) determine the average omega (sub 0) and alpha(sub abs) at each site (expanding upon previous work); (2) perform a sensitivity study on alpha(sub abs) by varying the spectral omega (sub 0); and (3) test the ability of each absorption and size relationship to distinguish aerosol types. The spectral omega (sub 0) averages indicate slightly more aerosol absorption (i.e., a 0.0 < delta omega (sub 0) <= 0.02 decrease) than in previous work and optical mixtures of pollution and smoke with dust show stronger absorption than dust alone. Frequency distributions of alpha(sub abs) show significant overlap among aerosol type categories and at least 10% of the alpha(sub abs) retrievals in each category are below 1.0. Perturbing the spectral omega (sub 0) by +/- 0.03 induces significant alpha(sub abs) changes from the unperturbed value by at least approx. +/- 0.6 for Dust, approx. +/-0.2 for Mixed, and approx. +/-0.1 for Urban/Industrial and Biomass Burning. The omega (sub 0)440nm and alpha(sub ext) 440-870nm relationship shows the best separation among aerosol type clusters, providing a simple technique for determining aerosol type from surface- and future space-based instrumentation.

Giles, David M.↗

NASA NTRS2014

Detection of High Velocity Absorption Components in the He I Lines of Eta Carinae near the Time of Periastron

We have obtained a total of 58 high spectral resolution (R90,000) spectra of the massive binary star eta Carinae since 2012 in an effort to continue our orbital and long-term echelle monitoring of this extreme binary (Richardson et al. 2010, AJ, 139, 1534) with the CHIRON spectrograph on the CTIO 1.5 m telescope (Tokovinin et al. 2013, PASP, 125, 1336) in the 45507500A region. We have increased our monitoring efforts and observation frequency as the periastron event of 2014 has approached. We note that there were multiple epochs this year where we observe unusual absorption components in the P Cygni troughs of the He I triplet lines. In particular, we note high velocity absorption components related to the following epochs for the following lines: He I 4713: HJD 2456754- 2456795 (velocity -450 to -560 kms) He I 5876: HJD 2456791- 2456819 (velocity -690 to -800 kms) He I 7065: HJD 2456791- 2456810 (velocity -665 to -730 kms) Figures: Note that red indicates a high-velocity component noted above. He I 4713: http:www.astro.umontreal.carichardson4713.png He I 5876: http:www.astro.umontreal.carichardson5876.png He I 7065: http:www.astro.umontreal.carichardson7065.png These absorptions are likely related to the wind-wind collision region and bow shock, as suggested by the high-velocity absorption observed by Groh et al. (2010, AA, 519, 9) in the He I 10830 Atransition. In these cases, we suspect that we look along an arm of the shock cone and that we will see a fast absorption change from the other collision region shortly after periastron. We suspect that this is related to the multiple-components of the He II 4686 line that was noted by Walter (ATel6334), and is confirmed in our data. Further, high spectral resolution data are highly encouraged,especially for resolving powers greater than 50,000.These observations were obtained with the CTIO 1.5 m telescope, operated by the SMARTS Consortium, and were obtained through both SMARTS and NOAO programs 2012A-0216,2012B-0194, and 2013b-0328). We thank Emily MacPherson (Yale) for her efforts in scheduling the observations that we have and will obtain in the coming weeks.

binary star eta Carinae↗

NASA NTRS2013

Portable 4.6 Micrometers Laser Absorption Spectrometer for Carbon Monoxide Monitoring and Fire Detection

The air quality aboard manned spacecraft must be continuously monitored to ensure crew safety and identify equipment malfunctions. In particular, accurate real-time monitoring of carbon monoxide (CO) levels helps to prevent chronic exposure and can also provide early detection of combustion-related hazards. For long-duration missions, environmental monitoring grows in importance, but the mass and volume of monitoring instruments must be minimized. Furthermore, environmental analysis beyond low-Earth orbit must be performed in-situ, as sample return becomes impractical. Due to their small size, low power draw, and performance reliability, semiconductor-laser-based absorption spectrometers are viable candidates for this purpose. To reduce instrument form factor and complexity, the emission wavelength of the laser source should coincide with strong fundamental absorption lines of the target gases, which occur in the 3 to 5 micrometers wavelength range for most combustion products of interest, thereby reducing the absorption path length required for low-level concentration measurements. To address the needs of current and future NASA missions, we have developed a prototype absorption spectrometer using a semiconductor quantum cascade laser source operating near 4.6 micrometers that can be used to detect low concentrations of CO with a compact single-pass absorption cell. In this study, we present the design of the prototype instrument and report on measurements of CO emissions from the combustion of a variety of aerospace plastics.

Tunable Environmental Laser Spectrometer (TELS)↗

NASA NTRSDate not supplied

Characterization Progress of an Absorption Laser Differential Interferometer

An absorption laser differential interferometer (A-LDI) system can be used to provide simultaneous, colinear measurements of flow properties (pressure, temperature, concentration, velocity) and flow fluctuations. Further characterization work on the absorption aspect of the system is provided in this paper, including characterization of the laser operating parameters, comparisons of two etalons of different free spectral range, and the further evaluation of a fixed-wavelength absorption measurement that can be used to obtain absorption and LDI measurements with the same sampling rate. A 0.4 GHz etalon was demonstrated to provide sufficient fringe peaks at low modulation depths to be used for the low-pressure testing characteristic of hypersonic wind tunnel facilities. The use of a 3 GHz etalon as a low-cost relative wavemeter was tested and validated. Data taken with the fixed-wavelength strategy in a sub-atmospheric test cell using 100% O2was successful and will allow absorption and LDI data to be acquired simultaneously, colinearly, and at the same sampling rate, yielding a truly simultaneous measurement of the flow density fluctuations and the flow mean density.

Joshua M Weisberger↗

NASA NTRSDate not supplied

Characterization Progress of an Absorption Laser Differential Interferometer

An absorption laser differential interferometer (A-LDI) system can be used to provide simultaneous, colinear measurements of flow properties (pressure, temperature, concentration, velocity) and flow fluctuations. Further characterization work on the absorption aspect of the system is provided in this paper, including characterization of the laser operating parameters, comparisons of two etalons of different free spectral range, and the further evaluation of a fixed-wavelength absorption measurement that can be used to obtain absorption and LDI measurements with the same sampling rate. A 0.4 GHz etalon was demonstrated to provide sufficient fringe peaks at low modulation depths to be used for the low-pressure testing characteristic of hypersonic wind tunnel facilities. The use of a 3 GHz etalon as a low-cost relative wavemeter was tested and validated. Data taken with the fixed-wavelength strategy in a sub-atmospheric test cell using 100% O 2 was successful and will allow absorption and LDI data to be acquired simultaneously, colinearly, and at the same sampling rate, yielding a truly simultaneous measurement of the flow density fluctuations and the flow mean density.

Joshua M. Weisberger↗

DOE OSTI2026

In-Band Scattering and Absorption of Infrared Blocking Foam Filters for Millimeter-wave Cameras

Expanded closed-cell polymer foams are widely used as thermal infrared (IR) blocking filters in millimeter-wave cameras, particularly for Cosmic Microwave Background observations. Precise knowledge of their millimeter-wave properties is essential for optimizing sensitivity. We present broadband (150 GHz - 2 THz) transmittance spectroscopy of Styroace-II and several Zotefoam filters, fitting their spectra with a radiative transfer model incorporating dielectric absorption and Rayleigh, Mie, and higher-order scattering. For a typical 5~cm thick filter stack at 280~GHz, Styroace-II exhibits ${\sim}10\%$ scattering with absorption estimated as ${\lesssim}5\%$ by effective-medium theory, while Zotefoam HD30 offers superior performance at ${\sim}3\%$ scattering and absorption likewise bounded to ${{\lesssim}0.3\%}$. Each model component is constrained at the ${\sim}0.1\%$ transmittance level for millimeter wavelengths. We observe batch-to-batch scattering variability of up to 2 percentage points in foams with multiple tested batches. Less commonly used Zotefoam formulations (LD15 and LD24) can further reduce in-band scattering to ${<}1\%$ while maintaining negligible in-band absorption and likely comparable IR blocking due to shared polyethylene absorption features and similar cell sizes. Based on this work, a filter constructed from the best measured LD24 batch has replaced the Styroace-II filter in a Simons Observatory 220/280 GHz Small Aperture Telescope.

Thomas, Alex [Chicago U., Astron. Astrophys. Ctr.;↗

DOE OSTI2023

Temporal Ni K-Edge X-ray Absorption Spectroscopy Study Reveals the Kinetics of the Ni Redox Behavior of the Iron-Nickel Oxide Bimetallic OER Catalyst

Operando X-ray absorption spectroscopy (XAS) can be utilized to probe the phase and structural changes of FeNiOx and similar transition metal oxide electrocatalysts during electrocatalytic reactions. However, capturing the temporal changes occurring in the operando chemistry of electrocatalysts has been little studied. Here, in this work, we successfully capture the time-resolved changes at the Ni K-edge for both the X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) regions of an aqueous phase synthesized FeNiO x bimetallic nanoparticle electrocatalyst. During a stepped voltage experiment, the temporal change in the Ni K-edge was observed as the applied voltage was stepped from 0.7 to 0.8 V versus the silver/silver chloride reference electrode, and the change observed is associated with the Ni redox transition from the 2+ to 3+/4+ oxidation state. Individual XAS spectra were obtained in 90 s, and a total of 9 scans post voltage step showed a unique transition from a hydroxide to an oxyhydroxide phase. The shift in absorption edge energy position and the changes in spectral shape for individual scans explain the typically observed broadening of the Ni K-edge XANES spectrum during time-averaged operando XAS, and a kinetic analysis revealed a first-order observed rate constant, |k obs |, of 0.00426 s –1 and a half-life (t 1/2 ) of 163 s. Multivariate curve resolution-alternating least squares analysis followed by linear combination fitting analysis for time-averaged versus time-resolved Ni K-edge changes upon voltage step show distinct differences in estimated contributions from Ni 2+ oxide/hydroxide phases. Detailed EXAFS modeling shows the phase transition from hydroxide to oxyhydroxide on top of the unchanged metallic core.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Excited-State Charge Distribution of a Donor–π–Acceptor Zn Porphyrin Probed by N K-Edge Transient Absorption Spectroscopy

Zinc porphyrin solar cell dyes with donor-π–acceptor architectures combine light absorber (π), electron-donor, and electron-acceptor moieties inside a single molecule with atomic precision. The donor-π–acceptor design promotes the separation of charge carriers following optical excitation. Here, we probe the excited-state electronic structure within such molecules by combining time-resolved X-ray absorption spectroscopy at the N K-edge with first-principles time-dependent density functional theory (TD-DFT) calculations. Furthermore, customized Zn porphyrins with strong-donor triphenylamine groups or weak-donor tri-tert-butylbenzene groups were synthesized. Energetically well-separated N K-edge absorption features simultaneously probe the excited-state electronic structure from the perspectives of the macrocycle and triphenylamine N atoms. New absorption transitions between the macrocycle N atoms and the excited-state HOMO vacancy are observed, and the triphenylamine associated absorption feature blue-shifts, consistent with partial oxidation of the donor groups in the excited state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser

Femtosecond carrier dynamics in layered 2H-MoTe2 semiconductor crystals have been investigated using soft x-ray transient absorption spectroscopy at the x-ray free-electron laser (XFEL) of the Pohang Accelerator Laboratory. Following above-bandgap optical excitation of 2H-MoTe2, the photoexcited hole distribution is directly probed via short-lived transitions from the Te 3d5/2 core level (M5-edge, 572–577 eV) to transiently unoccupied states in the valence band. The optically excited electrons are separately probed via the reduced absorption probability at the Te M5-edge involving partially occupied states of the conduction band. A 400 ± 110 fs delay is observed between this transient electron signal near the conduction band minimum compared to higher-lying states within the conduction band, which we assign to hot electron relaxation. Additionally, the transient absorption signals below and above the Te M5 edge, assigned to photoexcited holes and electrons, respectively, are observed to decay concomitantly on a 1–2 ps timescale, which is interpreted as electron–hole recombination. The present work provides a benchmark for applications of XFELs for soft x-ray absorption studies of carrier-specific dynamics in semiconductors, and future opportunities enabled by this method are discussed.

2D materials↗

DOE OSTI2024

Measurements of K-edge and L-edge extended x-ray absorption fine structure at the national ignition facility (invited)

High-energy-density laser facilities and advances in dynamic compression techniques have expanded access to material states in the Terapascal regime relevant to inertial confinement fusion, planetary science, and geophysics. However, experimentally determining the material temperature in these extreme conditions has remained a difficult challenge. Extended X-ray Absorption Fine Structure (EXAFS), referring to the modulations in x-ray absorption above an absorption edge from photoelectrons’ interactions with neighboring atoms, has proven to be a versatile and robust technique for probing material temperature and density for mid-to-high Z elements under dynamic compression. The current platform at the National Ignition Facility has developed six configurations for EXAFS measurements between 7 and 18 keV for different absorption edges (Fe K, Co K, Cu K, Ta L3, Pb L3, and Zr K) using a curved-crystal spectrometer and a bright, continuum foil x-ray source. Here, in this work, we describe the platform geometry, x-ray source performance, spectrometer resolution and throughput, design considerations, and data in ambient and dynamic-compression conditions.

36 MATERIALS SCIENCE↗

NASA NTRS2013

Absorption and Scattering by Molecules and Particles

The Earth's atmosphere absorbs, scatters, and emits electromagnetic radiation. Although air molecules are the primary actors in these processes, aerosol particles are also present ubiquitously and modify the radiation field. In fact, this modification constitutes the very physical basis of aerosol remote sensing. Whenever clouds are present, they have a much larger influence on radiation which largely overshadows the aerosol impact. Therefore, in aerosol remote sensing, one often has to limit observations to cloudless conditions and screen cloudy pixels. In the solar part of the spectrum, molecular absorption is mostly limited to ultraviolet (UV; ozone) and near-infrared (near-IR; carbon dioxide, water vapor) wavelengths and is characterized by strong and narrow oxygen bands. A brief description of atmospheric molecular absorption is presented in Section 2.2. Shortwave aerosol remote sensing is usually performed outside the absorption bands, but some instruments also have channels capturing absorption bands with the objective of quantifying gaseous components.

remote sensing↗

DOE OSTI2020

Self-absorption and Phonon Pulse Shape Discrimination in Scintillating Bolometers

In this work, we show that self-absorption of photons in scintillating bolometers can differentiate phonon pulse shapes between α (or nuclear recoil) and β/γ signals. This enables phonon pulse shape discrimination for particle identification. We establish a detector signal model that includes self-absorption and compare the simulated phonon pulse shapes with previously reported experimental results. The model predicts increase in pulse shape difference at higher self-absorption. Based on this result, we propose a new design of scintillating bolometers using 4π light reflectors for maximized self-absorption and only a single phonon readout, instead of light detectors that are typically employed for particle discrimination in scintillating bolometers.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2019

Electrospun Synthesis of Reduced Graphene Oxide (RGO)/NiZn Ferrite Nanocomposites for Excellent Microwave Absorption Properties

In this work, NiZn ferrite nanofibers were fabricated via electrospinning technique, followed by physical conversion into reduced graphene oxide (RGO)/NiZn ferrite nanocomposites. The whole graphene nanosheets were uniformly decorated with these magnetic nanocrystals without aggregation. The obtained ternary composite was characterized by various instruments for the chemical composition and microstructure. The results show that RGO/NiZn ferrite nanocomposites have remarkable improvements in both permittivity and permeability, which can be attributed to the combination of the good conductivity of light-weight graphene and high magnetocrystalline anisotropy of NiZn ferrites, thus significantly improving microwave absorption properties. With a matching thickness of only 2.0 mm, the reflection loss of superior sample of RGO/Ni{sub 0.7}Zn{sub 0.3}Fe{sub 2}O{sub 4} hybrid can reach − 37.71 dB at 12.5 GHz, and a reflection loss exceeding 10 dB absorption bandwidth can achieve 3.68 GHz. This indicates that the RGO/NiZn ferrite composite is an excellent and promising microwave absorbent with good absorption property, thin thickness, and wide absorption bandwidth.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2019

Enhancement of responsivity and speed in waveguide Ge/Si avalanche photodiode with separate vertical Ge absorption, lateral Si charge and multiplication configuration

Waveguide-coupled Ge/Si separate absorption, charge and multiplication avalanche photodiodes (SACM APDs) have shown significant potential as high-sensitivity, low-noise, and high-speed photo-detection for optical communications. Here we present a nanoscale single-mode waveguide-integrated vertical Ge absorption, lateral Si charge and single multiplication configuration for a waveguide Ge/Si SACM APD. This device can achieve 90% absorption at 1550 nm wavelengths with a 10 μm-long Ge layer. The device exhibits a seven times reduction in device length compared to conventional waveguide structures and a 29% increase compared to multi-mode interference coupling. Meanwhile, a 3-dB bandwidth can achieve 47 GHz, which is five times higher than the conventional vertical Ge absorption, lateral Si charge and multiplication devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2020

A microchannel shell-and-tube absorber for ammonia-water absorption

A shell-and-tube absorber with microscale geometric features that yields significant volumetric heat duties is investigated. A vertically-oriented baffled shell-and-tube heat exchanger with a tightly packed tube bundle is designed to serve as the absorber for a 10.5 kW nominal cooling capacity absorption chiller. The heat and mass transfer in this absorber is investigated experimentally at operating conditions spanning a wide range of working fluid and coupling fluid flow rates and ambient temperatures. An experimental facility is fabricated to closely simulate the operating conditions in an absorption refrigeration system. Absorption heat duties in the range of 5-15 kW are measured. In addition to operating the absorber in the baseline co-current flow configuration with premixed inlet, fluid ports are provided to enable operation in counter-current flow, where the dilute solution enters from the top and vapor enters from the bottom. The performance of these two flow configurations is compared. A preliminary heat and mass transfer model is developed to quantify the local temperatures, concentrations, and mass flow rates of the solution and vapor streams along the length of the absorber. The model predictions for total heat duty agree with the experimental results within 10% for almost all the data points, with an AAD of ~3.4%. Finally, the results of this study, along with the modeling framework, can guide further development of highly compact and efficient absorbers absorption systems.

42 ENGINEERING↗

DOE OSTI2021

Origin of the background absorption in carbon nanotubes: Phonon-assisted excitonic continuum

Excitonic effects in 1D semiconductors can be qualitatively different from those in higher dimensions. In particular, the Sommerfeld factor, the ratio of the above-band-edge excitonic continuum absorption to free electron-hole pair generation, has been shown to be less than 1 (suppressed) in 1D systems while it is larger than 1 (enhanced) in 2D and 3D systems. Strong continuum suppression indeed exists in semiconducting single-wall carbon nanotubes, a prototypical 1D semiconductor. However, absorption spectra for carbon nanotubes are typically fit with a combination of Lorentzians and a polynomial background baseline with little physical meaning. We performed absorption measurements in aligned single-chirality (6,5) carbon nanotube films. The obtained spectra were fit with our theoretical model obtained by solving the Boltzmann scattering equation involving fifty-nine different types of transitions among three different types of quasiparticles. Specifically, we took into account microscopic interactions between photons, phonons, and excitons, including their dispersions, which unambiguously demonstrated that the background absorption is due to phonon-assisted transitions from the semiconductor vacuum to finite-momentum continuum states of excitons. The excellent agreement we obtained between experiment and theory suggests that our numerical technique can be seamlessly extended to compute strongly out-of-equilibrium many-body dynamics and time-resolved spectra in low-dimensional materials.

36 MATERIALS SCIENCE↗